PETROLEUM PROCESSING AND PETROCHEMICALS ›› 2024, Vol. 55 ›› Issue (8): 74-83.

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Pd-LOADED CATALYST FOR CATALYTIC DECARBONYLATION OF DIMETHYL OXALATE TO PRODUCE DIMETHYL CARBONATE

  

  • Received:2024-01-17 Revised:2024-04-12 Online:2024-08-12 Published:2024-07-29

Abstract: In order to develop a high efficient and low cost synthetic process for dimethyl carbonate (DMC), supported Pd catalysts were prepared by impregnation method on Naβ(25), NaZSM-5(25), NaY(6), NaY(8),NaY(10) zeolites, and it was first used in the decarbonylation reaction of dimethyl oxalate (DMO). The composition, valence, pore structure, morphology and crystal of the catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy and Fourier transform infrared spectroscopy. The results showed that DMC was synthesized by the decarbonylation of DMO over Pd/NaY (6) catalyst. Under the optimum conditions such as a reaction temperature of 220 ℃,a reaction time of 90 min,a catalyst dosage of 1.0 g, a mass ratio of 1,4-dioxane to DMO of 4:1, and Pd loading 0.2%, the conversion of DMO and the selectivity of DMC were 82.59% and 62.33%, respectively. After five cycles of regeneration, the catalyst showed good catalytic activity for DMO decarboxylation. Finally, the reaction mechanism of DMC synthesis by DMO decarbonylation over Pd/NaY (6) catalyst was reasonably deduced.

Key words: zeolite, Pd catalyst, dimethyl oxalate, decarbonylation, dimethyl carbonate